Electrocatalytic Volleyball: Rapid Nanoconfined Nicotinamide Cycling for Organic Synthesis in Electrode Pores

In living cells, redox chains rely on nanoconfinement using tiny enclosures, such as the mitochondrial matrix or chloroplast stroma, to concentrate enzymes and limit distances that nicotinamide cofactors and other metabolites must diffuse. In a chemical analogue exploiting this principle, nicotinami...

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Bibliographic Details
Published in:Angewandte Chemie 2019-04, Vol.131 (15), p.5002-5006
Main Authors: Megarity, Clare F., Siritanaratkul, Bhavin, Heath, Rachel S., Wan, Lei, Morello, Giorgio, FitzPatrick, Sarah R., Booth, Rosalind L., Sills, Adam J., Robertson, Alexander W., Warner, Jamie H., Turner, Nicholas J., Armstrong, Fraser A.
Format: Article
Language:English
Subjects:
Chemistry
Chloroplasts
Cofactors
Electrode materials
Electrodes
Elektrokatalyse
Enzymes
Ferredoxin
Ferredoxin-NADP+-Reduktase
Indium tin oxides
Kofaktor-Rezyklierung
Metabolites
Mitochondria
NADP
NADPH-diaphorase
Nanoumgebung
Nicotinamid
Nicotinamide
Nicotinamide adenine dinucleotide
Organic chemistry
Pores
Reductase
Stroma
Tin
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Summary:In living cells, redox chains rely on nanoconfinement using tiny enclosures, such as the mitochondrial matrix or chloroplast stroma, to concentrate enzymes and limit distances that nicotinamide cofactors and other metabolites must diffuse. In a chemical analogue exploiting this principle, nicotinamide adenine dinucleotide phosphate (NADPH) and NADP+ are cycled rapidly between ferredoxin–NADP+ reductase and a second enzyme—the pairs being juxtaposed within the 5–100 nm scale pores of an indium tin oxide electrode. The resulting electrode material, denoted (FNR+E2)@ITO/support, can drive and exploit a potentially large number of enzyme‐catalysed reactions. Aus nächster Nähe: In den 5–100 nm großen Poren einer Indiumzinnoxid‐Elektrode werden NADPH und NADP+ durch eine Ferredoxin‐NADP+‐Reduktase (FNR) und ein Dehydrogenase‐Enzym (E2) rasch und reversibel ineinander umgewandelt. Die Elektrode ahmt die Nanoumgebung natürlicher Systeme nach, wie beispielsweise das Chloroplastenstroma oder die Mitochondrien in lebenden Zellen.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.201814370